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Abstract Precise modulating the vertical structure of active layers to boost charge transfer is an effective way to achieve high power conversion efficiencies (PCEs) in organic solar cells (OSCs). Herein, efficient OSCs with a well‐controlled vertical structure are realized by a rapid film‐forming method combining low boiling point solvent and the sequential blade‐coating (SBC) technology. The results of grazing incident wide‐angle X‐ray scattering measurement show that the vertical component distribution is varied by changing the processing solvent. Novel characterization technique such as tilt resonant soft X‐ray scattering is used to test the vertical structure of the films, demonstrating the dichloromethane (DCM)‐processed film is truly planar heterojunction. The devices with chloroform (CF) processed upper layer show an increased mixed phase region compared to these devices with toluene (TL) or ‐DCM‐, which is beneficial for improving charge generation and achieving a superior PCE of 17.36%. Despite significant morphological varies, the DCM‐processed devices perform slightly lower PCE of 16.66%, which is the highest value in truly planar heterojunction devices, demonstrating higher morphological tolerance. This work proposes a solvent‐regulating method to optimize the vertical structure of active layers through SBC technology, and provides a practical guidance for the optimization of the active‐layer microstructure. 

Printable and flexible organic solar panels are promising sources of inexpensive, large-scale renewable energy, where panels can be manufactured by printing from polymer inks. There are some limitations to these types of solar cells, however. First, toxic halogenated solvents have historically been necessary to dissolve polymers to make the ink. In addition, organic solar cells typically have high rates of recombination, which limits their efficiency. Here, we use a transient photovoltage (TPV) technique to measure charge lifetimes in cells made from two different organic solvents. The first solvent is toxic, halogenated dichlorobenzene (DCB) which is typically used to make organic solar cells. The other is a less toxic, non-halogenated solvent, carbon disulfide (CS2). By varying the processing methods in this way, we find that cells made from CS2 have longer charge lifetimes and higher efficiencies than those made with DCB, as well as a different recombination rate order. Possible reasons for these differences are explored using simple analytic modeling. Our model indicates that while bimolecular recombination is dominant in both types of cells, those processed with DCB may have more trap-assisted recombination present than those processed with CS2. Overall, this work demonstrates that we may be able to decrease the toxicity of organic solar cell manufacturing and simultaneously improve the efficiency of the devices, bringing this powerful method of capturing solar energy to the forefront of sustainable energy solutions.